The growing awareness of the pressing need for greener, more sustainable technologies has focused attention on the use of atom efficient catalytic methodologies for the manufacture of fine chemicals and pharmaceuticals. The use of alternative reaction solvents such as supercritical fluids or fluorous biphasic systems that are readily recycled has therefore become the focus of significant research that could circumvent the problems associated with many of the traditional volatile organic solvents. Thus novel and effective methods for reactor design, enzyme recovery and recycling are receiving increasing attention. New approaches to tackling these issues form the main objectives of this Proposal. The use of immobilized enzymes in the form of Cross-Linked Enzyme Aggregates (CLEAs) in supercritical carbon dioxide (scCO2) or fluorous reaction media including the use of ‘combi-CLEAs’, two enzymes that catalyse complementary reactions for one-pot two-step conversions in both batch and continuous reactions forms one major task. The use of hydrophobic-ion pairing of enzymes with perfluorinated surfactants to solubilise them in scCO2 and fluorous solvents and thus allow homogeneous catalysis to occur is the focus of the second task. The oxidases catalyzing the mild and clean formation of H2O2 from dioxygen will be investigated. This H2O2 will then be used in epoxidation and Baeyer-Villiger chemistry, either on the product of the oxidase reaction or a second substrate. Enzyme catalyzed polymerization reactions in scCO2 and fluorous solvents will also be investigated including the formation of perfluorinated polymers that may have unique physical and chemical properties. This fellowship will bring together strong research background of Dr. I. Lapenaite with excellent training opportunities at the University of Nottingham. This team aims to deliver significant breakthroughs in the development of new environmentally sustainable processing of organic materials.
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